The Novel Polymorphic Form of Bis(3,5,7-triaza-1-azoniatricyclo[ ]decane) bis( -oxo)-tris( -oxo)-nonakis( -oxo)-nonaaqua-decaoxo-hepta-molybdenum-di-zinc(II) dihydrate, Synthesis, and Properties
The reaction of molybdophosphoric acid with zinc carbonate followed by addition of hmta leads to formation of a triclinic polymorph of bis(3,5,7-triaza-1-azoniatricyclo[ ]decane) bis( -oxo)-tris( -oxo)-nonakis( -oxo)-nonaaqua-decaoxo-hepta-molybdenum-di-zinc(II) dihydrate in a one pot simple reaction. The obtained compound has been characterised by IR, UV-Vis spectroscopy, elemental analysis, and X-ray crystallography. A detailed comparison between both polymorphic forms: triclinic ？？, ？？, ？？, , , , and ？？3 and monoclinic ？？, ？？, ？？, , , , and ？？3 was performed. The influence of the synthesis procedure on polymorph formation was described. 1. Introduction The coordination chemistry of zinc is a field of growing interest from various viewpoints. The attention of scientists concentrates on synthetic aspects, structural, physicochemical properties, and reactivity of zinc compounds, as well as on their potential applications such as the development of catalysts (C–C bond formation reactions [1], carbon dioxide activation [2–4], etc.). Zinc complexes compounds are widely studied as biological mimics [5–7]. Zinc is an essential element for humans and is homeostatically regulated in the body. It has an important role in protein synthesis, and it is also a cofactor for many enzymes regulating cell growth and hormone levels, including regulation of gene transcription and growth factor metabolism [8]. Moreover, the mean zinc and lead concentrations in the human body correlate with the degree of urbanization and industrialization [9, 10]. Transition metal oxides such as molybdenum oxides are used in many industrial applications and have gained an interest from both technological and scientific points of view [11–15]. The main fields of industrial applications are catalysis, sorption, energy storage, molecular electronics, optical materials, and ceramics [16, 17]. Molybdenum oxides are an interesting example of this group of compounds and have a great industrial interest due to their optical and electronic properties. In fact, these transition metal oxides can be switched between two different optical states by photochromic, thermochromic, or electrochromic means [13]. Compounds that contain molybdenum oxides substructures modified by organonitrogen ligands were classified as a fifth class of oxides in which organic materials play a significant structural role [18]. Taking the above into consideration, there is a need for synthesis and investigations of new molybdenum cluster compounds. These compounds, containing additionally zinc cations, may possess interesting
References
[1]
T. Darbre and M. Machuqueiro, “Zn-proline catalyzed direct aldol reaction in aqueous media,” Chemical Communications, vol. 15, p. 1090, 2003.
[2]
D. J. Darensbourg, J. R. Wildeson, and J. C. Yarbrough, “Solid-state structures of zinc(II) benzoate complexes. Catalyst precursors for the coupling of carbon dioxide and epoxides,” Inorganic Chemistry, vol. 41, no. 4, pp. 973–980, 2002.
[3]
Y. Kawakami, K. Tajima, and T. Tsuruta, “Three-membered ring formation-IV. Selective syntheses of halogenocyclopropanedicarboxylic esters possessing different alcohol residues,” Tetrahedron, vol. 29, no. 9, pp. 1179–1183, 1973.
[4]
D. J. Darensbourg and M. S. Zimmer, “Copolymerization and terpolymerization of CO2 and epoxides using a soluble zinc crotonate catalyst precursor,” Macromolecules, vol. 32, no. 7, pp. 2137–2140, 1999.
[5]
B.-H. Ye, X.-Y. Li, I. D. Williams, and X.-M. Chen, “Synthesis and structural characterization of di- and tetranuclear zinc complexes with phenolate and carboxylate bridges. Correlations between 13C NMR chemical shifts and carboxylate binding modes,” Inorganic Chemistry, vol. 41, no. 24, pp. 6426–6431, 2002.
[6]
B. Singh, J. R. Long, F. Fabrizi De Biani, D. Gatteschi, and P. Stavropoulos, “Synthesis, reactivity, and catalytic behavior of iron/zinc-containing species involved in oxidation of hydrocarbons under Gif-type conditions,” Journal of the American Chemical Society, vol. 119, no. 30, pp. 7030–7047, 1997.
[7]
G. Parkin, “Synthetic analogues relevant to the structure and function of zinc enzymes,” Chemical Reviews, vol. 104, no. 2, pp. 699–767, 2004.
[8]
J. Brand？o-Neto, V. Stefan, B. B. Mendon？a, W. Bloise, and A. V. B. Castro, “The essential role of zinc in growth,” Nutrition Research, vol. 15, no. 3, pp. 335–358, 1995.
[9]
G. Fosse and N. P. B. Justesen, “Lead in deciduous teeth of Norwegian children,” Archives of Environmental Health, vol. 33, no. 4, pp. 166–175, 1978.
[10]
G. Fosse and N. P.B. Justesen, “Zinc and copper in deciduous teeth of Norwegian children,” International Journal of Environmental Studies, vol. 13, no. 1, pp. 19–34, 1978.
[11]
A. F. Wells, Structural Inorganic Chemistry, Oxford University Press, Oxford, UK, 1975.
[12]
N. N. Greenwood and A. Earnshaw, Chemistry of the Elements, Pergamon Press, New York, NY, USA, 1984.
[13]
G. E. Buono-Core, G. Cabello, A. H. Klahn et al., “Growth and characterization of molybdenum oxide thin films prepared by photochemical metal-organic deposition (PMOD),” Polyhedron, vol. 29, no. 6, pp. 1551–1554, 2010.
[14]
K. Bange, “Colouration of tungsten oxide films: a model for optically active coatings,” Solar Energy Materials and Solar Cells, vol. 58, no. 1, pp. 1–131, 1999.
[15]
A. Bouzidi, N. Benramdane, H. Tabet-Derraz, C. Mathieu, B. Khelifa, and R. Desfeux, “Effect of substrate temperature on the structural and optical properties of MoO3 thin films prepared by spray pyrolysis technique,” Materials Science and Engineering B, vol. 97, no. 1, pp. 5–8, 2003.
[16]
A. K. Cheetham, “Advanced inorganic materials: an open horizon,” Science, vol. 264, no. 5160, pp. 794–795, 1994.
[17]
P. A. Cox, Transition Metal Oxides, Clarendon Press, Oxford, UK, 1995.
[18]
P. J. Hagrman and J. Zubieta, “Solid-state coordination chemistry of metal oxides: hydrothermal synthesis and structural characterization of o-phenanthroline-ligated copper- and zinc-molybdenum oxides,” Inorganic Chemistry, vol. 38, no. 20, pp. 4480–4485, 1999.
[19]
A. Alamdari and F. Tabkhi, “Kinetics of hexamine crystallization in industrial scale,” Chemical Engineering and Processing, vol. 43, no. 7, pp. 803–810, 2004.
[20]
J. Altpeter, Das Hexamethylentetramin und Seine Verwendung, Knapp, 1931.
[21]
M. Svensson, L.A. Bengtsson-kloo, and H. Stegemann, “(Hexamethylenetetramine)diiodomercury(II), HgI2.hmt,” Acta Crystallographica Section C, vol. 51, pp. 2289–2292, 1995.
[22]
D. E. Bugay, “Characterization of the solid-state: spectroscopic techniques,” Advanced Drug Delivery Reviews, vol. 48, no. 1, pp. 43–65, 2001.
[23]
G. A. Stephenson, R. A. Forbes, and S. M. Reutzel-Edens, “Characterization of the solid state: quantitative issues,” Advanced Drug Delivery Reviews, vol. 48, no. 1, pp. 67–90, 2001.
[24]
D. J. W. Grant and H. Brittain, Eds., Polymorphism in Pharmaceutical Sciences, Drugs and the Pharmaceutical Sciences, Marcel Dekker, New York, NY, USA, 1999.
[25]
M. J. Pikal and H. Brittain, Eds., Polymorphism in Pharmaceutical Sciences, Drugs and the Pharmaceutical Sciences, Marcel Dekker, New York, NY, USA, 1999.
[26]
S. R. Byrn, R. R. Pfeiffer, and J. G. Stowell, Solid State Chemistry of Drugs, SSCI Incorporation, West Lafayette, Ind, USA, 2nd edition, 1999.
[27]
D. Singhal and W. Curatolo, “Drug polymorphism and dosage form design: a practical perspective,” Advanced Drug Delivery Reviews, vol. 56, no. 3, pp. 335–347, 2004.
[28]
J. Bernstein, J. D. Dunitz, and A. Gavezzotti, “Polymorphic perversity: crystal structures with many symmetry-independent molecules in the unit cell,” Crystal Growth and Design, vol. 8, no. 6, pp. 2011–2018, 2008.
[29]
G. S. Nichol and W. Clegg, “Further thoughts on crystal structures with : analysis of single-crystal structures determined using X-ray synchrotron and neutron radiation in the Cambridge Structural Database,” CrystEngComm, vol. 9, no. 10, pp. 959–960, 2007.
[30]
S. Aitipamula, G. R. Desiraju, M. Jaskólski, A. Nangia, and R. Thaimattam, “Multiple molecules in the crystallographic asymmetric unit. Self host-guest and doubly interpenetrated hydrogen bond networks in a pair of keto-bisphenols,” CrystEngComm, vol. 5, pp. 447–450, 2003.
[31]
R. Bishop and M. L. Scudder, “Multiple molecules in the asymmetric unit ( ) and the formation of false conglomerate crystal structures,” Crystal Growth and Design, vol. 9, no. 6, pp. 2890–2894, 2009.
[32]
K. M. Anderson, A. E. Goeta, and J. W. Steed, “Supramolecular synthon frustration leads to crystal structures with Z′ > 1,” Crystal Growth and Design, vol. 8, no. 7, pp. 2517–2524, 2008.
[33]
J. Minczewski and Z. Marczenko, Chemia Analityczna (eng. Analytical Chemistry), vol. 1, PWN, Warsaw, Poland, 1985.
[34]
X-RED. Version 1.18. STOE & Cie GmbH, Darmstadt, Germany, 1999.
[35]
G. M. Sheldrick, “A short history of SHELX,” Acta Crystallographica, vol. A64, no. 13, pp. 112–122, 2008.
[36]
F. J. Welcher, Analityczne Zastosowanie Kwasu Wersenowego (eng. The Analytical Uses of Etylenediamineteraacetic Acid), WNT, Warsaw, Poland, 1963.
[37]
Data Processing Module. Copyright ？ 1994–1998 SETARAM—FRANCE, Version 1.4.
[38]
T. Arumuganathan, A. Srinivasarao, T. V. Kumar, and S. K. Das, “Two different zinc(II)-aqua complexes held up by a metal-oxide based support: synthesis, crystal structure and catalytic activity of [HMTAH] 2[Zn(H2O)5Zn(H2O)4Mo7O24]·2H2O (HMTAH = protonated hexamethylenetetramine),” Journal of Chemical Sciences, vol. 120, no. 1, pp. 95–103, 2008.
[39]
T. He and J. Yao, “Photochromism of molybdenum oxide,” Journal of Photochemistry and Photobiology C, vol. 4, pp. 125–143, 2003.
[40]
M. Ainwar, C. A. Hogarth, and C. R. Theocharis, “A study of the infrared absorption spectra of thin amorphous films of molybdenum trioxide,” Journal of Materials Science, vol. 24, no. 7, pp. 2387–2390, 1989.
[41]
Z.-H. Zhou, H.-L. Wan, and K.-R. Tsai, “Molybdenum(VI) complex with citric acid: synthesis and structural characterization of 1？:？1 ratio citrato molybdate K2Na4[(MoO2)2O(cit)2]·5H2O,” Polyhedron, vol. 16, no. 1, pp. 75–79, 1997.
[42]
C. G. Barraclough, J. Lewis, and R. S. Nyholm, “The stretching frequencies of metal-oxygen double bonds,” Journal of the Chemical Society, pp. 3552–3555, 1959.
[43]
E. Guibal, C. Milot, O. Eterradossi, C. Gauffier, and A. Domard, “Study of molybdate ion sorption on chitosan gel beads by different spectrometric analyses,” International Journal of Biological Macromolecules, vol. 24, no. 1, pp. 49–59, 1999.
[44]
R. A. A. Muzzarelli, Chitin, Pergamon Press, Oxford, UK, 1977.
[45]
M. M. Miller and D. C. Sherrington, “Alkene epoxidations catalyzed by Mo(VI) supported on imidazole-containing polymers. I. Synthesis, characterization, and activity of catalysts in the epoxidation of cyclohexene,” Journal of Catalysis, vol. 152, no. 2, pp. 368–376, 1995.
[46]
R. A. Nyquist and R. O. Kagel, Infrared Spectra of Inorganic Compounds (3800–45 cm-1), Academic Press, London, UK, 1971.
[47]
M. Fournier, C. Louis, M. Che, P. Chaquin, and D. Masure, “Polyoxometallates as models for oxide catalysts. Part I. An UV-visible reflectance study of polyoxomolybdates: influence of polyhedra arrangement on the electronic transitions and comparison with supported molybdenum catalysts,” Journal of Catalysis, vol. 119, no. 2, pp. 400–414, 1989.
[48]
G. Xiong, C. Li, Z. Feng, P. Ying, Q. Xin, and J. Liu, “Surface coordination structure of molybdate with extremely low loading on γ-alumina characterized by UV resonance Raman spectroscopy,” Journal of Catalysis, vol. 186, no. 1, pp. 234–237, 1999.
[49]
T. Nowicka-Jankowska, UV-VIS Spectrophotometry in Chemical Analysis, PWN, Warszawa, Poland, 1988.
[50]
J. O. Jensen, “Vibrational frequencies and structural determinations of hexamethylenetetraamine,” Spectrochimica Acta—Part A, vol. 58, no. 7, pp. 1347–1364, 2002.
[51]
M. P. Bernstein, S. A. Sandford, L. J. Allamandola, and S. Chang, “Infrared spectrum of matrix-isolated hexamethylenetetramine in Ar and H2O at cryogenic temperatures,” Journal of Physical Chemistry, vol. 98, no. 47, pp. 12206–12210, 1994.
